All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane
In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d_{5/2}–σ^{*} transition of a gas-phase di-iodomethane (CH_{2}I_{2}) target. This site-specific excitation generates a 4d core hole located at an iodine site, which leaves the molecule in a well-...
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| Autores principales: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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| Formato: | article |
| Lenguaje: | EN |
| Publicado: |
American Physical Society
2021
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| Materias: | |
| Acceso en línea: | https://doaj.org/article/64b424a18119400eb2c7746afff63f50 |
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| Sumario: | In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d_{5/2}–σ^{*} transition of a gas-phase di-iodomethane (CH_{2}I_{2}) target. This site-specific excitation generates a 4d core hole located at an iodine site, which leaves the molecule in a well-defined excited state. We subsequently measure the time-dependent absorption change of the molecule with the FEL probe spectrum centered on the same I: 4d resonance. Using ab initio calculations of absorption spectra of a transient isomerization pathway observed in earlier studies, our time-resolved measurements allow us to assign the timescales of the previously reported direct and indirect dissociation pathways. The presented method is thus sensitive to excited-state molecular geometries in a time-resolved manner, following a core-resonant site-specific trigger. |
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